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Title: Interspace and Vacancy Modulation: Promoting the Zinc Storage of an Alcohol-Based Organic–Inorganic Cathode in a Water–Organic Electrolyte

Journal Article · · Advanced Materials
 [1];  [2];  [3];  [1];  [1];  [4];  [5];  [6]; ORCiD logo [7]
  1. Shandong Univ., Jinan (China)
  2. Renmin Univ. of China, Beijing (China)
  3. Swiss Federal Institute of Technology, Lausanne (Switzerland)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  5. Argonne National Laboratory (ANL), Argonne, IL (United States). X-ray Science Division
  6. Shandong Univ., Jinan (China); Qilu University of Technology, Jinan (China)
  7. Shandong Univ., Jinan (China); Qilu University of Technology, Jinan (China); Argonne National Laboratory (ANL), Argonne, IL (United States). X-ray Science Division
+ Show Author Affiliations

Abstract Expanding interspace and introducing vacancies are desired to promote the mobility of Zn ions and unlock the inactive sites of layered cathodes. However, this two‐point modulation has not yet been achieved simultaneously in vanadium phosphate. Here, a strategy is proposed for fabricating an alcohol‐based organic–inorganic hybrid material, VO 1− x PO 4 ·0.56C 6 H 14 O 4 , to realize the conjoint modulation of the d ‐interspace and oxygen vacancies. Peculiar triglycol molecules with an inclined orientation in the interlayer also boost the improvement in the conversion rate of V 5+ to V 4+ and the intensity of the PO bond. Their synergism can ensure steerable adjustment for intercalation kinetics and electron transport, as well as realize high chemical reactivity and redox‐center optimization, leading to at least 200% increase in capacity. Using a water–organic electrolyte, the designed Zn‐ion batteries with an ultrahigh‐rate profile deliver a long‐term durability (fivefold greater than pristine material) and an excellent energy density of ≈142 Wh kg −1 (including masses of cathode and anode), thereby substantially outstripping most of the recently reported state‐of‐the‐art zinc‐ion batteries. This work proves the feasibility to realize the two‐point modulation by using organic intercalants for exploiting high‐performance new 2D materials.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1991613
Alternate ID(s):
OSTI ID: 1893200
Journal Information:
Advanced Materials, Vol. 34, Issue 47; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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25 ENERGY STORAGE
Zn-ion batteries
d-interspaces
hybrid electrolytes
organic-inorganic materials
oxygen defects